Solution‐based thin‐film semiconductors offer a promising path for the mass production of low‐cost solar cells prepared at low temperatures. Thin‐film Cu‐based chalcogenides such as Cu(In,Ga)(S,Se)2 (CIGSSe) and Cu2ZnSn(S,Se)4 (CZTSSe) hold great promise and have been regarded as viable candidates because of the abundance of their constituent elements and environmentally nontoxic nature. This Review summarizes the recent progress in solution‐processed Cu chalcogenides (CuInSe2, Cu(In,Ga)(S,Se)2, Cu2ZnSnS4, Cu2ZnSn(S,Se)4) for thin‐film solar cells, with emphasis on the precursor solution deposited by spray pyrolysis and spin coating. The general aspects, current status, and recent research highlights are introduced and analyzed in detail. Finally, the challenges and future prospects of these solar cells are also discussed.
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